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Modeling colloid transport for performance assessment.

The natural system is expected to contribute to isolation at the proposed high-level nuclear waste (HLW) geologic repository at Yucca Mountain, NV (YM). In developing performance assessment (PA) computer models to simulate long-term behavior at YM, colloidal transport of radionuclides has been proposed as a critical factor because of the possible reduced interaction with the geologic media. Site-specific information on the chemistry and natural colloid concentration of saturated zone groundwaters in the vicinity of YM is combined with a surface complexation sorption model to evaluate the impact of natural colloids on calculated retardation factors (RF) for several radioelements of concern in PA. Inclusion of colloids into the conceptual model can reduce the calculated effective retardation significantly. Strongly sorbed radionuclides such as americium and thorium are most affected by pseudocolloid formation and transport, with a potential reduction in RF of several orders of magnitude. Radioelements that are less strongly sorbed under YM conditions, such as uranium and neptunium, are not affected significantly by colloid transport, and transport of plutonium in the valence state is only moderately enhanced. Model results showed no increase in the peak mean annual total effective dose equivalent (TEDE) within a compliance period of 10,000 years, although this is strongly dependent on container life in the base case scenario. At longer times, simulated container failures increase and the TEDE from the colloidal models increased by a factor of 60 from the base case. By using mechanistic models and sensitivity analyses to determine what parameters and transport processes affect the TEDE, colloidal transport in future versions of the TPA code can be represented more accurately.

Adsorption↗

Linking cesium and strontium uptake to kaolinite weathering in simulated tank waste leachate.

Weathering behavior of kaolinite was studied in batch systems under geochemical conditions characteristic of tank waste released to the vadose zone at the Hanford Site, WA (0.05 M Al(T), 2 M Na+, 1 M N03-, pH approximately 14, Cs+ and Sr2+ present as co-contaminants). Time series experiments were conducted from 0 to 369 d, with initial Cs+ and Sr2+ concentrations ranging from 10(-5) to 10(-3) M. Dissolution of kaolinite increased soluble Si and Al to maximum levels at 7 d (Cs and Sr concentrations of 10(-5) and 10(-4) M) or 33 d (Cs and Sr concentrations of 10(-3) M). Subsequent precipitation of Si and Al was coupled to the formation of oxalate-extractable solids that incorporated Cs and Sr. Strontium sorption was nearly complete within 24 h for initial Sr concentrations (Sr0) < or = 10(-4) whereas Cs uptake increased over the full year of the experiment for all initial Cs concentrations. Spectroscopic analyses revealed neoformed solids including the zeolite Na-Al silicate (Al-chabazite), and feldspathoids sodium aluminum nitrate silicate (NO3-sodalite), and sodium aluminum nitrate silicate hydrate (NO3-cancrinite), which can incorporate Cs. Single-pulse 27Al solid-state nuclear magnetic resonance (NMR) spectroscopyyielded first-order rate constants (k)for mineral transformation that decreased from 3.5 x 10(-3) to 2 x 10(-3) d(-1) as Cs and Sr concentrations were increased from 10(-5) to 10(-3) M. Discrete strontium silicate solids were also observed. The incongruent dissolution of kaolinite promoted the sequestration of contaminants into increasingly recalcitrant solid phases over the 1-yr time period.

Adsorption↗

Time-resolved laser fluorescence spectroscopy study of the sorption of Cm(III) onto smectite and kaolinite.

For long-term performance assessment of nuclear waste repositories knowledge concerning interactions of actinides with mineral surfaces is imperative. The mobility and bioavailability of released radionuclides is strongly dependent on sorption/desorption processes onto mineral surfaces. Therefore it is necessary to characterize the surface species formed and to elucidate the reaction mechanisms involved. The high fluorescence spectroscopic sensitivity of Cm(III) has attracted our interest regarding the complexation process of Cm(III) onto smectite and kaolinite as a model system for the sorption of trivalent actinides in the trace concentration range. We conclude that at low pH Cm(III) is sorbed onto kaolinite and smectite as an outer-sphere complex and retains its complete primary hydration sphere. With increasing pH inner-sphere adsorption onto kaolinite and smectite occurs via the aluminol edge sites. The same evolution of the Cm(III)-clay surface species as a function of pH was observed for both minerals. Starting at a pH > or = 5 we observe the formation of a [triple bond]Al-O-Cm2+(H2O)5 surface complex, which is replaced by a second species at higher pH. The second surface complex may be a monodentate [triple bond]Al-O-Cm+(OH)(H2O)4 species or bidentate [triple bond](Al-O)2-Cm+(H2O)5 species. The Cm(III)/clay surface complexes are characterized bytheir emission spectra (peak maxima at 598.8 and 603.3 nm) and their fluorescence lifetime (both 110 +/- 7 micros). An important result in view of the mobility and bioavailability of radionuclides is that no incorporation of Cm(III) into the bulk clay structure was observed.

Adsorption↗

A reaction-transport model for calcite precipitation and evaluation of infiltration fluxes in unsaturated fractured rock.

The percolation flux in the unsaturated zone (UZ) is an important parameter addressed in site characterization and flow and transport modeling of the potential nuclear-waste repository at Yucca Mountain, NV, USA. The US Geological Survey (USGS) has documented hydrogenic calcite abundances in fractures and lithophysal cavities at Yucca Mountain to provide constraints on percolation fluxes in the UZ. The purpose of this study was to investigate the relationship between percolation flux and measured calcite abundances using reactive transport modeling. Our model considers the following essential factors affecting calcite precipitation: (1) infiltration, (2) the ambient geothermal gradient, (3) gaseous CO(2) diffusive transport and partitioning in liquid and gas phases, (4) fracture-matrix interaction for water flow and chemical constituents, and (5) water-rock interaction. Over a bounding range of 2-20 mm/year infiltration rate, the simulated calcite distributions capture the trend in calcite abundances measured in a deep borehole (WT-24) by the USGS. The calcite is found predominantly in fractures in the welded tuffs, which is also captured by the model simulations. Simulations showed that from about 2 to 6 mm/year, the amount of calcite precipitated in the welded Topopah Spring tuff is sensitive to the infiltration rate. This dependence decreases at higher infiltration rates owing to a modification of the geothermal gradient from the increased percolation flux. The model also confirms the conceptual model for higher percolation fluxes in the fractures compared to the matrix in the welded units, and the significant contribution of Ca from water-rock interaction. This study indicates that reactive transport modeling of calcite deposition can yield important constraints on the unsaturated zone infiltration-percolation flux and provide useful insight into processes such as fracture-matrix interaction as well as conditions and parameters controlling calcite deposition.

Calcium Carbonate↗

Aluminum effect on dissolution and precipitation under hyperalkaline conditions: I. Liquid phase transformations.

Substantial amounts of self-boiling, Al-rich, hyperalkaline, and saline high-level waste fluids (HLWF) were deposited to the vadose zone at the Hanford Site, in Washington State. The objective of this study was to investigate the effects of similar fluids on the extent of dissolution and precipitation in the sediments. Metal- and glass-free systems were used to conduct batch experiments at 323 K under CO2 and O2 free conditions. Base-induced dissolution of the soil minerals was rapid in the first 48 h as indicated by immediate releases of Si and Fe into the soil solution. Potassium release lagged behind and dissolution of K-bearing minerals (mica and K-feldspar) proceeded faster only after 2 to 3 d of the experiment. Silicon and Fe release exhibited high dependence on aqueous [Al] (rate orders <-1), because Al decreased free OH concentration in the contact solution and probably inhibited soil mineral dissolution. Initial K release exhibited low dependence on [Al] (fractional rate orders). Initial dissolution rates calculated based on Si release varied with aqueous [Al] from 29.47 to 4.35 x 10(-12) mol m(-2) s(-1). Aluminum participated in the formation of the secondary phases (precipitation rates of 10(-8) mol s(-1)) but the overall precipitation rate of alumino-silicate secondary phases was probably controlled by aqueous [Si] (rates of 10(-9), and rate constants between 0.0054 and 0.0084 h(-1)). The changes in the soil solution chemistry (release of K, Si, Fe, and other elements) may play a significant role in the fate of radionuclides and contaminants like Cs, Sr, Cr, and U in the Hanford sediments.

Accidents↗

Effect of coupled dissolution and redox reactions on Cr(VI)aq attenuation during transport in the sediments under hyperalkaline conditions.

Aluminum-rich, hyperalkaline (pH > 13.5) and saline high-level nuclear waste (HLW) fluids at elevated temperatures (>50 degrees C), that possibly contained as much as 0.41 mol L(-1) Cr(VI), accidentally leaked to the sediments at the Hanford Site, WA. These extreme conditions promote base-induced dissolution of soil minerals which may affect Cr(VI)aq mobility. Our objective was to investigate Cr(VI)aq transport in sediments leached with HLW simulants at 50 degrees C, under CO2 and O2 free conditions. Results demonstrated that Cr(VI)aq fate was closely related to dissolution, and Cr(VI)aq mass loss was negligible in the first pore volumes but increased significantly thereafter. Similar to dissolution, Cr(VI)aq attenuation increased with increasing fluid residence time and NaOH concentration but decreased with Al concentrations in the leaching solutions. Aqueous Cr(VI) removal rate half-lives varied from 1.2 to 230 h with the fastest at the highest base concentration, lowest Al concentration, greatest reaction time, and lowest Cr(VI) concentration in the leaching solution. The rate of Cr(VI) removal (normalized to 1 kg of solution) varied from 0.83 x 10(-9) (+/-0.44 x 10(-9)) to 9.16 x 10(-9) (+/-1.10 x 10(-9)) mol s(-1). The predominant mechanism responsible for removing Cr(VI) from the aqueous phase appears to be homogeneous Cr(VI) reduction to Cr(III) by Fe(II) released during mineral dissolution. Cr(VI)aq removal was time-limited probably because it was controlled by the rate of Fe(II) release into the soil solution upon mineral dissolution, which was also a time-limited process, and other processes that may act to lower Fe(II)aq activity.

Carcinogens, Environmental↗

Microbial impacts to the near-field environment geochemistry: a model for estimating microbial communities in repository drifts at Yucca Mountain.

Geochemical and microbiological modeling was performed to evaluate the potential quantities and impact of microorganisms on the geochemistry of the area adjacent to and within nuclear waste packages in the proposed repository drifts at Yucca Mountain, Nevada. The microbial growth results from the introduction of water, ground support, and waste package materials into the deep unsaturated rock. The simulations, which spanned 1 million years, were accomplished using a newly developed computer code, Microbial Impacts to the Near-Field Environment Geochemistry (MING). MING uses environmental thresholds for limiting microbial growth to temperatures below 120 degrees C and above relative humidities of 90% in repository drifts. Once these thresholds are met, MING expands upon a mass balance and thermodynamic approach proposed by McKinley et al. [FEMS Microbiol. Rev. 20 (1997) 545] by using kinetic rates to supply constituents from design materials and constituent fluxes including solubilized rock components into the drift to perform two separate mass balance calculations as a function of time. The first (nutrient limit) assesses the available nutrients (C, N, P and S) and calculates how many microorganisms can be produced based on a microorganism stoichiometry of C(160)(H(280)O(80))N(30)P(2)S. The second (energy limit) calculates the energy available from optimally combined redox couples for the temperature and pH at that time. This optimization maximizes those reactions that produce >15 kJ/mol (limit on useable energy) using an iterative linear optimization technique. The final available energy value is converted to microbial mass at a rate of 1 kg of biomass (dry weight) for every 64 MJ of energy. These two values (nutrient limit and energy limit) are then compared and the smaller value represents the number of microorganisms that can be produced over a specified time. MING can also be adapted to investigate other problems of interest as the model can be used in saturated and unsaturated environments and in laboratory situations to establish microbial growth limitations. Other projected uses include investigations of contaminated locations where monitored natural attenuation or engineered bioremediation could be employed.

Carbon↗

Explosion investigation of asphalt-salt mixtures in a reprocessing plant.

Cause investigation of a fire and explosion at the nuclear fuel waste reprocessing plant indicated that self-heating ignition of an asphalt-salt-waste, bituminized, mixture (AS) caused the disaster. A 220l drum was filled with the AS at a temperature of about 180 degrees C. About 20h later the drum ignited and burned as it was being cooled. It is estimated that the AS contained approximately 55wt.% blown asphalt, 25wt.% NaNO(3), 5wt.% NaNO(2), 8wt.% Na(2)CO(3), 2wt.% NaH(2)PO(4), 1wt.% Ba (OH)(2), 1wt.% K(4)[Fe(CN)(6)], and possibly 3wt.% of other materials. To determine the reaction promoting factors and pertinent chemical reaction rates, self-reaction of the AS has been investigated by the use of a C80D heat flux reaction calorimeter. The oxidizing reactions with asphalt are ruled by NaNO(2) rather than by NaNO(3), in spite of a lower concentration of NaNO(2). The kinetic rates of the interfacial reaction between salt particles and asphalt for the reaction controlled and diffusion controlled steps have been formulated as a function of salt particle size for both NaNO(2) and NaNO(3). Numerical solution of the heat balance equations formulating the heterogeneous reaction scheme indicates that a runaway reaction occurs when the AS-filling temperature is 208 degrees C for a drum filled with an AS mixture produced under standard operating conditions. Molecules containing intramolecular hydrogen, such as Na(2)HPO(4) and NaHCO(3), do not oxidize asphalt directly, however, their presence chemically promotes the oxidizing reaction of NaNO(2). Moreover, NaHCO(3) decomposition which produces gases creates many micro holes in the interior of the salt particles. This in turn promotes the oxidizing reactions that are diffusion controlled. Finally, the consequence of a runaway reaction at 180 degrees C or lower is qualitatively explained by taking into account the chemical effect of intramolecular hydrogen and the physical effect of the NaHCO(3) decomposition gases.

Explosions↗

Performance assessments of nuclear waste repositories: a dialogue on their value and limitations.

Performance Assessment (PA) is the use of mathematical models to simulate the long-term behavior of engineered and geologic barriers in a nuclear waste repository; methods of uncertainty analysis are used to assess effects of parametric and conceptual uncertainties associated with the model system upon the uncertainty in outcomes of the simulation. PA is required by the U.S. Environmental Protection Agency as part of its certification process for geologic repositories for nuclear waste. This paper is a dialogue to explore the value and limitations of PA. Two "skeptics" acknowledge the utility of PA in organizing the scientific investigations that are necessary for confident siting and licensing of a repository; however, they maintain that the PA process, at least as it is currently implemented, is an essentially unscientific process with shortcomings that may provide results of limited use in evaluating actual effects on public health and safety. Conceptual uncertainties in a PA analysis can be so great that results can be confidently applied only over short time ranges, the antithesis of the purpose behind long-term, geologic disposal. Two "proponents" of PA agree that performance assessment is unscientific, but only in the sense that PA is an engineering analysis that uses existing scientific knowledge to support public policy decisions, rather than an investigation intended to increase fundamental knowledge of nature; PA has different goals and constraints than a typical scientific study. The "proponents" describe an ideal, six-step process for conducting generalized PA, here called probabilistic systems analysis (PSA); they note that virtually all scientific content of a PA is introduced during the model-building steps of a PSA; they contend that a PA based on simple but scientifically acceptable mathematical models can provide useful and objective input to regulatory decision makers. The value of the results of any PA must lie between these two views and will depend on the level of knowledge of the site, the degree to which models capture actual physical and chemical processes, the time over which extrapolations are made, and the proper evaluation of health risks attending implementation of the repository. The challenge is in evaluating whether the quality of the PA matches the needs of decision makers charged with protecting the health and safety of the public.

Geological Phenomena↗

Fluid flow and reactive transport around potential nuclear waste emplacement tunnels at Yucca Mountain, Nevada.

The evolution of fluid chemistry and mineral alteration around a potential waste emplacement tunnel (drift) is evaluated using numerical modeling. The model considers the flow of water, gas, and heat, plus reactions between minerals, CO(2) gas, and aqueous species, and porosity-permeability-capillary pressure coupling for a dual permeability (fractures and matrix) medium. Two possible operating temperature modes are investigated: a "high-temperature" case with temperatures exceeding the boiling point of water for several hundred years, and a "low-temperature" case with temperatures remaining below boiling for the entire life of the repository. In both cases, possible seepage waters are characterized by dilute to moderate salinities and mildly alkaline pH values. These trends in fluid composition and mineral alteration are controlled by various coupled mechanisms. For example, upon heating and boiling, CO(2) exsolution from pore waters raises pH and causes calcite precipitation. In condensation zones, this CO(2) redissolves, resulting in a decrease in pH that causes calcite dissolution and enhances feldspar alteration to clays. Heat also enhances dissolution of wall rock minerals leading to elevated silica concentrations. Amorphous silica precipitates through evaporative concentration caused by boiling in the high-temperature case, but does not precipitate in the low-temperature case. Some alteration of feldspars to clays and zeolites is predicted in the high-temperature case. In both cases, calcite precipitates when percolating waters are heated near the drift. The predicted porosity decrease around drifts in the high-temperature case (several percent of the fracture volume) is larger by at least one order of magnitude than in the low temperature case. Although there are important differences between the two investigated temperature modes in the predicted evolution of fluid compositions and mineral alteration around drifts, these differences are largely within to the model uncertainty and the variability of water compositions at Yucca Mountain.

Carbon Dioxide↗

The incidence of childhood leukaemia around the La Hague nuclear waste reprocessing plant (France): a survey for the years 1978-1998.

BACKGROUND: A previous study has suggested an increased incidence rate of leukaemia from 1978 to 1992 in people aged 0 to 24 years and living in the vicinity of the La Hague nuclear waste reprocessing plant without considering age and cytological type. SETTING: The Nord Cotentin region (France) and the island of Alderney (United Kingdom). STUDY OBJECTIVE: To describe the occurrence of leukaemia for each age group and cytological type from 1978 to 1998 in the same area, using accurate reference incidence rates and adequate estimation of the at risk population. DESIGN: A geographical study of incidence using three zones defined according to their distance from the site (0 to 10 km: Beaumont-Hague electoral ward, 10 to 20 km and 20 to 35 km) has been conducted. The risk of leukaemia was estimated from the standardised incidence ratio (SIR) of the number of cases observed to the number expected. Exact 95% confidence intervals (CI) have been computed. PARTICIPANTS: All people under the age of 25 years living in the study region between 1978 and 1998. MAIN RESULTS: The observed number of cases of leukaemia in the study region as a whole was consistent with the expected value (SIR=1.03; 95%CI: 0.73, 1.41). No cases were observed on Alderney. The SIR in the Beaumont-Hague electoral ward was 2.17 (95%CI: 0.71, 5.07). The highest SIR was observed in the 5 to 9 years age group (SIR=6.38; 95%CI: 1.32, 18.65). This consists in acute lymphoblastic leukaemia cases. CONCLUSION: This study indicates an increased incidence of leukaemia in the area situated at less than 10 km from the plant. Monitoring and further investigations should be targeted at acute lymphoblastic leukaemia occurring during the childhood incidence peak (before 10 years) in children living near the La Hague site and may be other nuclear reprocessing plants.

Adolescent↗

Interpretation of actinide-distribution data obtained from non-destructive and destructive post-test analyses of an intact-core column of Culebra dolomite.

The US Department of Energy (DOE), with technical assistance from Sandia National Laboratories, has successfully received EPA certification and opened the Waste Isolation Pilot Plant (WIPP), a nuclear waste disposal facility located approximately 42 km east of Carlsbad, NM. Performance assessment (PA) analyses indicate that human intrusions by inadvertent, intermittent drilling for resources provide the only credible mechanisms for significant releases of radionuclides from the disposal system. For long-term brine releases, migration pathways through the permeable layers of rock above the Salado formation are important. Major emphasis is placed on the Culebra Member of the Rustler Formation because this is the most transmissive geologic layer overlying the WIPP site. In order to help quantify parameters for the calculated releases, radionuclide transport experiments have been carried out using intact-core columns obtained from the Culebra dolomite member of the Rustler Formation within the WIPP site. This paper deals primarily with results of analyses for 241Pu and 241Am distributions developed during transport experiments in one of these cores. Transport experiments were done using a synthetic brine that simulates Culebra brine at the core recovery location (the WIPP air-intake shaft (AIS)). Hydraulic characteristics (i.e., apparent porosity and apparent dispersion coefficient) for intact-core columns were obtained via experiments using the conservative tracer 22Na. Elution experiments carried out over periods of a few days with tracers 232U and 239Np indicated that these tracers were weakly retarded as indicated by delayed elution of the species. Elution experiments with tracers 241Pu and 241Am were attempted but no elution of either species has been observed to date, including experiments of many months' duration. In order to quantify retardation of the non-eluted species 241Pu and 241Am after a period of brine flow, non-destructive and destructive analyses of one intact-core column were carried out to determine distribution of these actinides in the rock. Analytical results indicate that the majority of the 241Am remained very near the injection surface of the core (possibly as a precipitate), and that the majority of the 241Pu was dispersed with a very high apparent retardation value. The 241Pu distribution is interpreted using a single-porosity advection-dispersion model, and an approximate retardation value is reported.

Actinoid Series Elements↗

239,240Pu and inorganic substances in aerosols from the vicinity of a waste isolation pilot plant: the importance of resuspension.

Aerosol samples were collected and analyzed to characterize the spatial and temporal variations in the concentrations of plutonium and selected inorganic substances in the atmosphere around the Waste Isolation Pilot Plant (WIPP). High-volume aerosol sampling was conducted at three sites: (1) On Site, (2) Near Field, and (3) Cactus Flats. 239,240Pu was determined by alpha spectrometry following chemical separations; mass loadings were determined gravimetrically. A separate set of low-volume aerosol samples was analyzed for major ions using ion chromatography and for trace elements by inductively-coupled plasma emission spectrometry and mass spectrometry. The average 239,240Pu activity concentrations in total suspended particle (TSP) samples (12 to 16 nBq m(-3)) were consistent with those previously reported, but they varied strongly with season, with the highest values generally in spring. Further, the 239,240Pu activity concentrations were comparable among the three sites, and therefore there was no evidence for elevated 239,240Pu activities due to WIPP operations. The fraction of the 239,240Pu activity concentrations in the PM10, samples (particles less than 10 microm diameter) relative to TSP was lower than the corresponding PM10/TSP ratios of either high-volume mass or several inorganics (sulfate, aluminum or lead), indicating that 239,240Pu tends to be on large particles. Aerosol mass loadings (microg m(-3)) and 239,240Pu activity concentrations were correlated for all sets of samples, but at On Site, the TSP samples showed higher mass to 239,240Pu ratios than the other sites. Thus activities or processes occurring at or near the WIPP site evidently produced aerosols that contributed to the mass loadings but contained less 239,244Pu than ambient aerosols. About 63% of the variability in 239,240Pu activity concentrations was explained by wind travel, sampling location, length of the sampling interval, and aerosol mass. 239,240Pu activity concentrations also were correlated with aluminum (an indicator of mineral dust), further implicating the resuspension of soils as an important determinant of 239,240Pu in aerosols. The 239,240Pu/Al ratios for the aerosols were higher than in soils, and this could be explained by the preferential binding of 239,240Pu to small soil particles that have large surface area to mass ratios and also have higher aluminum contents than larger particles.

Aerosols↗

Residual waste from Hanford tanks 241-C-203 and 241-C-204. 2. Contaminant release model.

Release of U and 99Tc from residual sludge in Hanford waste tanks 241-C-203 and 241-C-204 atthe U.S. Department of Energy's (DOE) Hanford Site in southeastern Washington state was quantified by water-leaching, selective extractions, empirical solubility measurements, and thermodynamic modeling. A contaminant release model was developed based on these experimental results and solid-phase characterization results presented elsewhere. Uranium release was determined to be controlled by two phases and occurred in three stages. In the first stage, U release is controlled by the solubility of tejkaite, which is suppressed by high concentrations of sodium released from the dissolution of NaNO3 in the residual sludges. Equilibrium solubility calculations indicate the U released during this stage will have a maximum concentration of 0.021 M. When all the NaNO3 has dissolved from the sludge, the solubility of the remaining cejkaite will increase to 0.28 M. After cejkaite has completely dissolved, the majority of the remaining U is in the form of poorly crystalline Na2U2O7 [or clarkeite Na[(UO2)O(OH)](H20)0-1]. In contact with Hanford groundwater this phase is not stable, and becquerelite becomes the U solubility controlling phase, with a calculated equilibrium concentration of 1.2 x 10(-4) M. For Tc, a significant fraction of its concentration in the residual sludge was determined to be relatively insoluble (20 wt % for C-203 and 80 wt % for C-204). Because of the low concentrations of Tc in these sludge materials, the characterization studies did not identify any discrete Tc solids phases. Release of the soluble fraction of Tc was found to occur concomitantly with NO3-. It was postulated that a NaNO3-NaTcO4 solid solution could be responsible for this behavior. The Tc release concentrations for the soluble fraction were estimated to be 2.4 x 10-6 M for C-203 and 2.7 x 10(-5) M for C-204. Selective extraction results indicated that the recalcitrant fraction of Tc was associated with Fe oxides. Release of the recalcitrant fraction of Tc was assumed to be controlled by dissolution of Fe oxide in the form of ferrihydrite. Based on this assumption and measured values for the ratio of recalcitrant Tc to total Fe in each bulk sludge, the release concentration of the recalcitrant fraction of Tc was calculated to be 3.9 x 10(-12) M for C-203 and 10.0 x 10(-12) M for C-204.

Radioactive Waste↗

Neutron analysis of spent fuel storage installation using parallel computing and advance discrete ordinates and Monte Carlo techniques.

In the United States, the Nuclear Waste Policy Act of 1982 mandated centralised storage of spent nuclear fuel by 1988. However, the Yucca Mountain project is currently scheduled to start accepting spent nuclear fuel in 2010. Since many nuclear power plants were only designed for -10 y of spent fuel pool storage, > 35 plants have been forced into alternate means of spent fuel storage. In order to continue operation and make room in spent fuel pools, nuclear generators are turning towards independent spent fuel storage installations (ISFSIs). Typical vertical concrete ISFSIs are -6.1 m high and 3.3 m in diameter. The inherently large system, and the presence of thick concrete shields result in difficulties for both Monte Carlo (MC) and discrete ordinates (SN) calculations. MC calculations require significant variance reduction and multiple runs to obtain a detailed dose distribution. SN models need a large number of spatial meshes to accurately model the geometry and high quadrature orders to reduce ray effects, therefore, requiring significant amounts of computer memory and time. The use of various differencing schemes is needed to account for radial heterogeneity in material cross sections and densities. Two P3, S12, discrete ordinate, PENTRAN (parallel environment neutral-particle TRANsport) models were analysed and different MC models compared. A multigroup MCNP model was developed for direct comparison to the SN models. The biased A3MCNP (automated adjoint accelerated MCNP) and unbiased (MCNP) continuous energy MC models were developed to assess the adequacy of the CASK multigroup (22 neutron, 18 gamma) cross sections. The PENTRAN SN results are in close agreement (5%) with the multigroup MC results; however, they differ by -20-30% from the continuous-energy MC predictions. This large difference can be attributed to the expected difference between multigroup and continuous energy cross sections, and the fact that the CASK library is based on the old ENDF/B-II library. Both MC and SN calculations were run in parallel on a BEOWULF PC-cluster (eight processors). Timing results indicate that the SN calculation yielded a detailed dose distribution at over 318,426 points in -164 h. Unbiased continuous energy MC required 214 h to calculate dose rates with a 1% relative error in only 18 regions on the surface of the cask. The biased A3MCNP calculations yields dose rates with -0.8% relative error in only 2.5 h on one processor. This study demonstrates that a parallel code, such as the 3-D parallel SN transport code, PENTRAN can solve a complex large problem, such as the storage cask, accurately and efficiently. Moreover, this calculation was performed on a relatively inexpensive PC-cluster. Possible inadequacies of the CASK cross section library still need to be evaluated.

Computer-Aided Design↗

Health impacts of large releases of radionuclides. Roles of micro-organisms in the environmental fate of radionuclides.

Micro-organisms play important roles in the environmental fate of radionuclides in both aquatic and terrestrial ecosystems, with a multiplicity of physico-chemical and biological mechanisms effecting changes in mobility and speciation. Physico-chemical mechanisms of removal, which may be encompassed by the general term 'biosorption', include adsorption, ion exchange and entrapment. These are features of living and dead organisms as well as their derived products. In living cells biosorptive processes can be directly and indirectly influenced by metabolism, and may be reversible and affected by changing environmental conditions. Metabolism-dependent mechanisms of radionuclide immobilization include metal precipitation as sulfides, sequestration by metal-binding proteins and peptides, and transport and intracellular compartmentation. Chemical transformations of radionuclide species, particularly by reduction, can result in immobilization. Microbial processes involved in solubilization include autotrophic and heterotrophic leaching, complexation by siderophores and other metabolites, and chemical transformations. Such mechanisms are important components of natural biogeochemical cycles for radionuclides and should be considered in any analyses of environmental radionuclide contamination. Several micro-organism-based biotechnologies, e.g. those based on biosorption or precipitation, are of potential use for the treatment of radionuclide contamination.

Adsorption↗

The influence of the hair cycle on the thickness of mouse skin.

The data on mouse skin thickness reported here was prompted by the need to know the true position of basal cells of the epidermis and hair follicles as these are important "cells at risk" for a variety of skin reactions including carcinogenesis following exposure to radiation. There is little reliable data in the literature and most previous reports have ignored the shrinkage of skin that occurs because of its natural elasticity. The values determined for mouse flank skin in telogen--the resting phase of the hair cycle for the different skin layers--are epidermis 10 micron, corium 250 micron, adipose layer 150 micron, and hair follicle depth 150 micron. Three days after chemical depilation which triggers the hair follicles into active cycle (anagen) the epidermis doubles in thickness, remains at this value for 7 days, and then gradually returns to telogen values by day 18. The corium and adipose layers also increase significantly to reach approximately 390 micron and approximately 260 micron, respectively, by day 10 and then return to control values from day 15 onward. The change in hair follicles depths are more dramatic with active follicle basal cells reaching approximately 450-550 micron into the adipose layer between days 7 and 15. One important finding is that chemical depilation does not affect the telogen thickness of skin-the teleogen values for the epidermis and dermis immediately prior to and immediately after depilation were similar to those 23 days later at the beginning of the next telogen phase.

Animals↗

Depleted uranium--the growing concern.

Recently, several studies have reported on the health and environmental consequences of the use of depleted uranium. Depleted uranium is a heavy metal that is also radioactive. It is commonly used in missiles as a counterweight because of its very high density (1.6 times more than lead). Immediate health risks associated with exposure to depleted uranium include kidney and respiratory problems, with conditions such as kidney stones, chronic cough and severe dermatitis. Long-term risks include lung and bone cancer. Several published reports implicated exposure to depleted uranium in kidney damage, mutagenicity, cancer, inhibition of bone, neurological deficits, significant decrease in the pregnancy rate in mice and adverse effects on the reproductive and central nervous systems. Acute poisoning with depleted uranium elicited renal failure that could lead to death. The environmental consequences of its residue will be felt for thousands of years. It is inhaled and passed through the skin and eyes, transferred through the placenta into the fetus, distributed into tissues and eliminated in urine. The use of depleted uranium during the Gulf and Kosovo Wars and the crash of a Boeing airplane carrying depleted uranium in Amsterdam in 1992 were implicated in a health concern related to exposure to depleted uranium.

Animals↗